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In general, which is currently the better choice? I'm genuinely sat on the middle of the fence here. From what I understand the usual setup is a valkyrie with a vet squad loaded with melta or plasma, or a vendetta with a melta special weapons squad, but which of these is the more all-rounder choice? I'm leaning more towards the valkyrie for the lower points cost and ability to carry a full vet squad, but 3 TL las sounds nice too.

They fit different roles.

The valk is an anti-infantry air support transport(rocket pods and multilaser are the true default loadouts, hb may be addrd but not necessary)

The vendetta is an airsuperiority fighter that happens to have some tranport capacity.

It is completely a case of one shoots vehicles/mc/gmc and the other shoots non-vehicles

melta vets.. they are on a suicide mission to blow up something important.

put em in a vendetta and have a great anti-armor combo

Vendetta with meltas/demos or Command squad with flammers.

Plasma Special Weapons Squad in a Vendetta. Drop them to kill Crisis Suits or MEQs as the Brutal Fangs of the TL-Las Skewer that LR/Monolith/FMC/GMC/MC...

@OP: Valk is nice, but the Vendetta actually brings something to your list that will make it stronger overall.